Ultra-narrow room-temperature emission from single CsPbBr3 perovskite quantum dots

Gabriele Rainò*, Nuri Yazdani, Simon C. Boehme, Manuel Kober-Czerny, Chenglian Zhu, Franziska Krieg, Marta D. Rossell, Rolf Erni, Vanessa Wood, Ivan Infante, Maksym V. Kovalenko

*Corresponding author for this work

Research output: Contribution to JournalArticleAcademicpeer-review

Abstract

Semiconductor quantum dots have long been considered artificial atoms, but despite the overarching analogies in the strong energy-level quantization and the single-photon emission capability, their emission spectrum is far broader than typical atomic emission lines. Here, by using ab-initio molecular dynamics for simulating exciton-surface-phonon interactions in structurally dynamic CsPbBr3 quantum dots, followed by single quantum dot optical spectroscopy, we demonstrate that emission line-broadening in these quantum dots is primarily governed by the coupling of excitons to low-energy surface phonons. Mild adjustments of the surface chemical composition allow for attaining much smaller emission linewidths of 35−65 meV (vs. initial values of 70–120 meV), which are on par with the best values known for structurally rigid, colloidal II-VI quantum dots (20−60 meV). Ultra-narrow emission at room-temperature is desired for conventional light-emitting devices and paramount for emerging quantum light sources.

Original languageEnglish
Article number2587
Pages (from-to)1-8
Number of pages8
JournalNature Communications
Volume13
DOIs
Publication statusPublished - 2022

Bibliographical note

Funding Information:
G.R. acknowledges B. Benin and Dr. M. Bodnarchuk for useful discussions. M.V.K. acknowledges financial support from the Swiss Innovation Agency (Innosuisse, grant 32908.1 IP-EE) and, in part, from the European Union through Horizon 2020 research and innovation program (grant agreement No. [819740], project SCALE-HALO). I.I. acknowledges The Netherlands Organization of Scientific Research (NWO) for financial support through the Innovational Research Incentive (Vidi) Scheme (Grant No. 723.013.002) and S.C.B. acknowledges NWO for financial support through the Innovational Research Incentives (Veni) Scheme (Grant No. 722.017.011). N.Y. and V.W. acknowledge the Swiss National Supercomputing Centre (CSCS; project ID s1003). Funding for N.Y. was provided by the Swiss National Science Foundation through the Quantum Sciences and Technology NCCR. The project was also partially supported by the Air Force Office of Scientific Research and the Office of Naval Research under award number FA8655-21-1-7013, by the by the European Union’s Horizon 2020 program, through a FET Open research and innovation action under the grant agreement Grant No. 899141 (PoLLoC) and by the Swiss National Science Foundation (Grant No. 188404, “Novel inorganic light emitters: synthesis, spectroscopy and applications”).

Funding Information:
G.R. acknowledges B. Benin and Dr. M. Bodnarchuk for useful discussions. M.V.K. acknowledges financial support from the Swiss Innovation Agency (Innosuisse, grant 32908.1 IP-EE) and, in part, from the European Union through Horizon 2020 research and innovation program (grant agreement No. [819740], project SCALE-HALO). I.I. acknowledges The Netherlands Organization of Scientific Research (NWO) for financial support through the Innovational Research Incentive (Vidi) Scheme (Grant No. 723.013.002) and S.C.B. acknowledges NWO for financial support through the Innovational Research Incentives (Veni) Scheme (Grant No. 722.017.011). N.Y. and V.W. acknowledge the Swiss National Supercomputing Centre (CSCS; project ID s1003). Funding for N.Y. was provided by the Swiss National Science Foundation through the Quantum Sciences and Technology NCCR. The project was also partially supported by the Air Force Office of Scientific Research and the Office of Naval Research under award number FA8655-21-1-7013, by the by the European Union’s Horizon 2020 program, through a FET Open research and innovation action under the grant agreement Grant No. 899141 (PoLLoC) and by the Swiss National Science Foundation (Grant No. 188404, “Novel inorganic light emitters: synthesis, spectroscopy and applications”).

Publisher Copyright:
© 2022, The Author(s).

Funding

G.R. acknowledges B. Benin and Dr. M. Bodnarchuk for useful discussions. M.V.K. acknowledges financial support from the Swiss Innovation Agency (Innosuisse, grant 32908.1 IP-EE) and, in part, from the European Union through Horizon 2020 research and innovation program (grant agreement No. [819740], project SCALE-HALO). I.I. acknowledges The Netherlands Organization of Scientific Research (NWO) for financial support through the Innovational Research Incentive (Vidi) Scheme (Grant No. 723.013.002) and S.C.B. acknowledges NWO for financial support through the Innovational Research Incentives (Veni) Scheme (Grant No. 722.017.011). N.Y. and V.W. acknowledge the Swiss National Supercomputing Centre (CSCS; project ID s1003). Funding for N.Y. was provided by the Swiss National Science Foundation through the Quantum Sciences and Technology NCCR. The project was also partially supported by the Air Force Office of Scientific Research and the Office of Naval Research under award number FA8655-21-1-7013, by the by the European Union’s Horizon 2020 program, through a FET Open research and innovation action under the grant agreement Grant No. 899141 (PoLLoC) and by the Swiss National Science Foundation (Grant No. 188404, “Novel inorganic light emitters: synthesis, spectroscopy and applications”). G.R. acknowledges B. Benin and Dr. M. Bodnarchuk for useful discussions. M.V.K. acknowledges financial support from the Swiss Innovation Agency (Innosuisse, grant 32908.1 IP-EE) and, in part, from the European Union through Horizon 2020 research and innovation program (grant agreement No. [819740], project SCALE-HALO). I.I. acknowledges The Netherlands Organization of Scientific Research (NWO) for financial support through the Innovational Research Incentive (Vidi) Scheme (Grant No. 723.013.002) and S.C.B. acknowledges NWO for financial support through the Innovational Research Incentives (Veni) Scheme (Grant No. 722.017.011). N.Y. and V.W. acknowledge the Swiss National Supercomputing Centre (CSCS; project ID s1003). Funding for N.Y. was provided by the Swiss National Science Foundation through the Quantum Sciences and Technology NCCR. The project was also partially supported by the Air Force Office of Scientific Research and the Office of Naval Research under award number FA8655-21-1-7013, by the by the European Union’s Horizon 2020 program, through a FET Open research and innovation action under the grant agreement Grant No. 899141 (PoLLoC) and by the Swiss National Science Foundation (Grant No. 188404, “Novel inorganic light emitters: synthesis, spectroscopy and applications”).

FundersFunder number
FET Open research and innovation action188404
Innovational Research Incentives722.017.011
Office of Naval ResearchFA8655-21-1-7013
Air Force Office of Scientific Research
Horizon 2020 Framework Programme899141
European Commission
Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung
Nederlandse Organisatie voor Wetenschappelijk Onderzoek723.013.002
Horizon 2020819740
National Center of Competence in Research Quantum Science and Technology
Innosuisse - Schweizerische Agentur für Innovationsförderung32908.1 IP-EE
Centro Svizzero di Calcolo Scientificos1003

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